Based On The Construction Of Polypyridine Supramolecules And Their Catalytic Properties

Supramolecular chemistry,as a subject of studying non covalent bonding,has attracted more and more attention.Among various non covalent bond interactions,self-assembly driven by metal coordination bond has the advantages of directionality and controllability,and is widely used in the construction of supramolecules.Among many ligands,nitrogen-containing organic ligands occupy most of the supramolecular assembly in this field.From monodentate,bidentate to tridentate ligands,the self-assembly of monodentate pyridyl ligands and bidentate bipyridyl ligands has achieved fruitful development in the past few decades.Among them 2,2':6',2"-terpyridine is a tridentate chelating ligand,which has many excellent physical and chemical properties compared with other coordination systems.In recent years,researchers have successfully synthesized and reported a large number of controllable two-dimensional and three-dimensional supramolecules based on tripyridine;At present,researchers have constructed two-dimensional and three-dimensional supramolecules with aesthetic significance based on tripyridine,but the simple and beautiful structure can not meet the research needs of researchers.At present,more diversification and functionalization are the development trend of metal organic complexes of tripyridine.This paper mainly includes the following three works:(1)In Chapter 2,the photosensitive"V"type tripyridine ligand L1 was synthesized.Through the metal organic ligand synthesis strategy,the metal organic ligand L5 with six uncoordinated tripyridine was synthesized,which was self-assembled with Zn²⁺to form triangle S1.S1 was characterized by NMR,MS,TEM,UV-vis and fluorescence spectra,and the oxidative degradation of pollutant methyl sulfide was realized.(2)In Chapter 3,the"V"type tripyridine ligand with crown ether group was synthesized,and the triangular S2 of all metal ruthenium was formed by self-assembly with Ru²⁺.On the basis of"V"type tripyridine with crown ether,the metal organic ligand L4 was synthesized,and the triangular supramolecule S3 was formed by self-assembly of L4 and Zn2+.S2 and S3 were characterized by NMR,MS and TEM.S2was specifically identified with the catalytic center of pyridine salt with N+,and the catalytic center was enriched to form a three-dimensional cylindrical structure with two triangles and three catalytic centers.The formation process was studied by NMR titration,and its electrocatalytic oxidation was tested.(3)In Chapter 4,organic ligands were synthesized by one-step coupling reaction and self-assembled with Fe²⁺to form a tetrahedral structure S4.S4 was characterized by NMR,MS and TEM,and the formation process of tetrahedron was studied.The experimental results showed that the dipyridine part of the ligand first formed a dimer with Fe²⁺,and then the dipyridine part of the dimer coordinated with Fe²⁺to form a tetrahedral structure.